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Synergic Effects of Surface Chemistry and Applied Potentials on the Kinetics of the Electrocatalytic Oxygen Evolution Reaction in IrO2

Journal Article · · ACS Applied Energy Materials
 [1];  [1];  [1];  [2];  [2];  [3]
  1. Nanjing University of Science and Technology (China)
  2. Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
  3. Nanjing University of Science and Technology (China); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
+ Show Author Affiliations
Improving the efficacy of the oxygen evolution reaction (OER) through water oxidation is critical for advancing photoelectrochemical water splitting. Among the catalysts, IrO2 exhibits a high OER catalytic activity and stability under acidic conditions. The OER mechanism in this system has been a topic of intense research; however, many mechanistic understandings are lacking. In this work, we carried out first-principles calculations with an implicit solvation model at a constant potential to study the OER behavior on the IrO2(110) surface. We find that the surface hydrogen coverage has a significant effect on OER kinetics and transition states. We then develop a microkinetics model that accounts for the continuous evolution of both OER activation energy and hydrogen coverage as a function of an applied potential. We show that this inclusion leads to significant improvement in the simulated Tafel plot compared to available experiments. In conclusion, our results point to a complex interplay between surface chemistry and the applied potential on OER kinetics.
Research Organization:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Organization:
Natural Science Foundation of Jiangsu Province (NJUST); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)
Grant/Contract Number:
AC02-05CH11231; AC52-07NA27344
OSTI ID:
2282837
Report Number(s):
LLNL--JRNL-859620; 1090245
Journal Information:
ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 23 Vol. 6; ISSN 2574-0962
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

08 HYDROGEN
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Tafel slope
grand-canonical density functional theory
iridium oxides
oxygen evolution reaction
polarization current simulation
the first-principles simulation